LC-MS/MS method for quantitation of the CK2 inhibitor silmitasertib (CX-4945) in human plasma, CSF, and brain tissue, and application to a clinical pharmacokinetic study in children with brain tumors

J Chromatogr B Analyt Technol Biomed Life Sci. 2020 Sep 1:1152:122254. doi: 10.1016/j.jchromb.2020.122254. Epub 2020 Jun 23.

Abstract

Silmitasertib (CX-4945) as a potent and selective inhibitor of CK2 exhibited promising in vitro and in vivo anti-cancer activity. An assay employing cation-exchange solid phase extraction (SPE) followed by LC-MS/MS analysis was successfully developed and validated for the quantitation of silmitasertib in human plasma, brain tissue, and human cerebrospinal fluid (CSF). Reverse phase chromatographic separation was achieved using Synergi™ hydro-RP column (4 μm, 75 × 2.0 mm) and gradient elution with 5 mM ammonium formate aqueous solution (pH 6.5) as mobile phase A and 0.1% formic acid in acetonitrile as mobile phase B. Multiple reaction monitoring (MRM) transition of m/z 350.2 → 223.2 and m/z 316.2 → 223.2 were chosen for detection of silmitasertib and internal standard (CX-4786) respectively. Since silmitasertib concentration in patient plasma is expected to be in a wide range due to the study design, two calibration curves with range 0.2-125 ng/ml and 32-20,000 ng/ml were established. A different curve ranging from 2 to 40 ng/g was used for measurement of silmitasertib in brain tissue, while another calibration curve ranging from 0.2 to 20 ng/ml was established for CSF. All these calibration curves corresponding to different matrices showed good linearity (R2 > 0.99) over the concentration range. This assay demonstrated excellent precision below 15% and accuracies between 85% and 115% within-day and between-day for all the concentration levels in each matrix. This assay was also validated for each matrix for selectivity, sensitivity, matrix effects, recovery, and stability. We applied the validated method to the analysis of plasma silmitasertib for a clinical study.

Keywords: Brain tissue homogenate; CK2; CX-4945; Cation-exchange solid phase extraction; Human CSF; Human plasma; LC-MS/MS; Silmitasertib.

Publication types

  • Clinical Trial, Phase II

MeSH terms

  • Animals
  • Antineoplastic Agents / analysis*
  • Antineoplastic Agents / pharmacokinetics
  • Antineoplastic Agents / pharmacology
  • Antineoplastic Agents / therapeutic use
  • Brain / metabolism
  • Brain Chemistry / drug effects
  • Brain Neoplasms / drug therapy*
  • Child
  • Chromatography, High Pressure Liquid / methods
  • Chromatography, Reverse-Phase / methods*
  • Drug Stability
  • Humans
  • Limit of Detection
  • Linear Models
  • Macaca fascicularis
  • Macaca mulatta
  • Mice
  • Naphthyridines / analysis*
  • Naphthyridines / pharmacokinetics
  • Naphthyridines / pharmacology
  • Naphthyridines / therapeutic use
  • Phenazines / analysis*
  • Phenazines / pharmacokinetics
  • Phenazines / pharmacology
  • Phenazines / therapeutic use
  • Reproducibility of Results
  • Tandem Mass Spectrometry / methods*

Substances

  • Antineoplastic Agents
  • Naphthyridines
  • Phenazines
  • silmitasertib